Organic subcells are an essential component of organic-perovskite
tandem solar cells, yet current choices are limited to those with
low open-circuit voltages (V
OCs) and efficiencies.
By designing and synthesizing benzo[d][1,2,3]triazole-substituted
acceptors, LBz-F and LBz-Cl, which exhibit shallower frontier orbital
energy levels and narrower optical bandgaps than the typical nonfullerene
acceptor L8-BO, we overcome this limitation. LBz-F and LBz-Cl can
form alloys with L8-BO in the active layer, broadening the absorption,
optimizing charge carrier dynamics, and reducing energy losses of
the devices, which results in improved short-circuit currents and
fill factors without compromising a high V
OC in the organic subcell. By combining PM6:L8-BO:LBz-F as the back
cell with a wide bandgap (1.72 eV) perovskite front cell, efficiencies
of 22.11% and 20.18% with high V
OCs approaching
2.1 V are achieved for small and large area tandem devices, respectively,
highlighting the effectiveness of rational organic subcell engineering
for efficient, large-area organic-perovskite tandem solar cells.